2D氮化碳: 通过调节非金属硼掺杂C3N5阐明宽酸性及碱性pH范围的光催化析氢的反应机理

doi:10.1016/S1872-2067(23)64417-1

催化学报 ›› 2023, Vol. 47: 150-160.DOI: 10.1016/S1872-2067(23)64417-1

2D氮化碳: 通过调节非金属硼掺杂C₃N₅阐明宽酸性及碱性pH范围的光催化析氢的反应机理

Sue-Faye Ng^a^,^b, 陈星竹^c, Joel Jie Foo^a^,^b, 熊墨^d,*(), Wee-Jun Ong^a^,^b^,^e^,^f^,^g,*()

^a厦门大学马来西亚分校能源与化学工程学院, 雪兰莪, 马来西亚
^b厦门大学马来西亚分校纳米能源与催化技术卓越中心(CONNECT), 雪兰莪, 马来西亚
^cKAUST催化中心, 阿卜杜拉国王科技大学, 吉达, 沙特阿拉伯
^d西安交通大学物理学院, 教育部物质非平衡合成与调控重点实验室, 陕西西安710049, 中国
^e固体表面物理化学国家重点实验室, 厦门大学化学化工学院, 福建厦门361005, 中国
^f厦门大学深圳研究院, 广东深圳518057, 中国
^g厦门大学古雷石化研究院, 福建漳州363216, 中国

收稿日期:2022-12-28 接受日期:2023-02-08 出版日期:2023-04-18 发布日期:2023-03-20
通讯作者: *电子信箱: weejun.ong@xmu.edu.my (W.-J. Ong),xiongmo@xjtu.edu.cn (熊墨).
基金资助:
马来西亚高等教育部 (MOHE)“基础研究基金”(FRGS/1/2020/TK0/XMU/02/1);马来西亚科学、技术和创新部 (MOSTI)“战略研究基金"(SRF-APP);马来西亚科学、技术和创新部 (MOSTI)“战略研究基金"(S.22015);国家自然科学基金委(22202168);广东省基础与应用基础研究基金(2021A1515111019);厦门大学马来西亚分校研究基金(IENG/0038);厦门大学马来西亚分校的启动资助(ICOE/0001);厦门大学马来西亚分校的启动资助(XMUMRF/2021-C8/IENG/0041);厦门大学马来西亚分校的启动资助(XMUMRF/2019-C3/IENG/0013)

2D carbon nitrides: Regulating non-metal boron-doped C₃N₅ for elucidating the mechanism of wide pH range photocatalytic hydrogen evolution reaction

Sue-Faye Ng^a^,^b, Xingzhu Chen^c, Joel Jie Foo^a^,^b, Mo Xiong^d,*(), Wee-Jun Ong^a^,^b^,^e^,^f^,^g,*()

^aSchool of Energy and Chemical Engineering, Xiamen University Malaysia, Selangor Darul Ehsan 43900, Malaysia
^bCenter of Excellence for NaNo Energy & Catalysis Technology (CONNECT), Xiamen University Malaysia, Selangor Darul Ehsan 43900, Malaysia
^cKAUST Catalysis Center, King Abdullah University of Science and Technology, Thuwal 23955-6900, Saudi Arabia
^dMOE Key Laboratory for Non-Equilibrium Synthesis and Modulation of Condensed Matter, School of Physics, Xi’an Jiaotong University, Xi’an 710049, Shaanxi, China
^eState Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China
^fShenzhen Research Institute of Xiamen University, Shenzhen 518057, Guangdong, China
^gGulei Innovation Institute, Xiamen University, Zhangzhou 363216, Fujian, China

Received:2022-12-28 Accepted:2023-02-08 Online:2023-04-18 Published:2023-03-20
Contact: *E-mail: weejun.ong@xmu.edu.my (W.-J. Ong),xiongmo@xjtu.edu.cn (M. Xiong).
About author:Wee-Jun Ong (School of Energy and Chemical Engineering, Xiamen University Malaysia) received his B.Eng. and Ph.D. in chemical engineering from Monash University. He is presently an Assistant Dean and Associate Professor in the School of Energy and Chemical Engineering at Xiamen University Malaysia (XMUM). From 2016 to 2018, he was a scientist at Institute of Materials Research and Engineering (IMRE), Agency for Science, Technology and Research (ASTAR) in Singapore. Starting from 2021, he becomes a Director of the Center of Excellence for NaNo Energy & Catalysis Technology (CONNECT) at XMUM. In 2019, he was a visiting scientist at Technische Universität Dresden, Germany and a visiting professor at Lawrence Berkeley National Laboratory (LBNL), USA. His research interests focus on tunable design of nanostructured materials (i.e., 2D nanoarchitectures and carbon-based substrates) for photocatalytic, photoelectrocatalytic, and electrochemical H₂O splitting, CO₂ reduction, N₂ fixation and alcohol oxidation. Apart from these, his most recent progresses include the 3D printing nanotechnology as well as microwave plasma methane cracking for graphene and hydrogen production/storage. He has coauthored more than 120 peer-reviewed papers and received over 16000 citations and a H-index of 56 to date.
Supported by:
Ministry of Higher Education (MOHE) Malaysia under the Fundamental Research Grant Scheme (FRGS)(FRGS/1/2020/TK0/XMU/02/1);Ministry of Science, Technology and Innovation (MOSTI) Malaysia under the Strategic Research Fund(SRF-APP);Ministry of Science, Technology and Innovation (MOSTI) Malaysia under the Strategic Research Fund(S.22015);National Natural Science Foundation of China(22202168);Guangdong Basic and Applied Basic Research Foundation(2021A1515111019);Xiamen University Malaysia Investigatorship Grant(IENG/0038);Xiamen University Malaysia Research Fund(ICOE/0001);Xiamen University Malaysia Research Fund(XMUMRF/2021-C8/IENG/0041)

摘要/Abstract

摘要：

太阳能驱动水裂解产氢是一种绿色能源技术, 用于制备可再生和零碳排放燃料以实现可持续能源生产. 近期, 氮化碳(g-C₃N₄)同素异形体C₃N₅的出现克服了g-C₃N₄的固有缺点, 如光生载流子快速复合和可见光吸收差, 而导致极低的光催化效率.

本文将硼掺杂剂通过原子替换或间隙掺杂的方式引入到C₃N₅体系中, 并利用密度泛函理论对纯C₃N₅和硼掺杂C₃N₅体系进行计算, 考察了硼原子对C₃N₅电子和光学性能的影响以及其催化析氢反应(HER)机理. 热力学计算结果表明, 硼原子掺杂在C₃N₅体系中是可行且有利的. 在N3位氮原子被硼原子取代(B_N3-C₃N₅)后, 带隙(0.6 eV)变窄. 与纯C₃N₅相比, 硼掺杂剂通过Volmer Tafel和Volmer Heyrovsky机制降低了酸性和碱性介质中HER反应中决定步骤的反应能垒. B_N3-C₃N₅表面的氢吸附吉布斯自由能 (0.11 eV)与Pt/C催化剂(‒0.09 eV)相当. 综上, 非金属掺杂碳可提高氮化物的催化性能, 对未来该方向研究提供一定借鉴.

关键词: 氮化碳, 同素异形体, 析氢反应, 密度泛函理论, 酸性介质, 碱性介质, 光催化

Abstract:

Solar-driven water splitting for green hydrogen production has been prospected as an auspicious technology to achieve sustainable energy generation by shifting towards renewable and zero-carbon emission fuels. Recently, N-rich C₃N₅ allotropes are emerging to surpass the intrinsic drawbacks of g-C₃N₄, which are the rapid recombination of photogenerated charge carriers and poor visible light absorption, resulting in low photocatalytic efficiency. In this study, density functional theory calculation was conducted on the pristine C₃N₅ and boron-doped C₃N₅ systems to study the effect of boron atom on the electronic and optical properties, as well as the hydrogen evolution reaction mechanism. The boron-dopants were introduced in C₃N₅ through substitutional or interstitial doping. It is indicated that the incorporation of boron atoms in the C₃N₅ matrix is thermodynamically favorable. A band gap narrowing of 0.6 eV was observed after the N3-site nitrogen atom was replaced by a boron atom (B_N3-C₃N₅). Compared to pristine C₃N₅, the boron-dopant also reduced the reaction energies of potential determining step of the HER pathway in both acid and alkaline media through the Volmer-Tafel and Volmer-Heyrovsky mechanism. The Gibbs free energy of hydrogen adsorption (ΔG_H*) of B_N3-C₃N₅ (0.11 eV) is comparable to the benchmark Pt/C catalyst (-0.09 eV). These theoretical results allude to the elucidated catalytic performance of non-metal doped carbon nitrides that can be applied to future experimental and computational analysis.

Key words: Carbon nitride, Allotrope, Hydrogen evolution reaction, Density functional theory, Acidic media, Alkaline media, Photocatalysis

Sue-Faye Ng, 陈星竹, Joel Jie Foo, 熊墨, Wee-Jun Ong. 2D氮化碳: 通过调节非金属硼掺杂C₃N₅阐明宽酸性及碱性pH范围的光催化析氢的反应机理[J]. 催化学报, 2023, 47: 150-160.

Sue-Faye Ng, Xingzhu Chen, Joel Jie Foo, Mo Xiong, Wee-Jun Ong. 2D carbon nitrides: Regulating non-metal boron-doped C₃N₅ for elucidating the mechanism of wide pH range photocatalytic hydrogen evolution reaction[J]. Chinese Journal of Catalysis, 2023, 47: 150-160.

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图/表 10

Fig. 1. Top and side view of g-C3N4 (a) and triazole-triazine C3N5 (b) framework marked with positions used for boron-doping. The C and N atoms are represented in brown and grey, respectively.

Fig. 2. Formation energies of boron-dopant on various sites on C3N5. The C, N and boron atoms are represented in brown, grey, and green, respectively.

Table 1 Work function (Φ) of boron-doped C3N5 and pristine C3N5 models.

Model	W_F (Φ)
B_C1-C₃N₅	5.71
B_N2-C₃N₅	5.76
B_N3-C₃N₅	5.02
B_N4-C₃N₅	5.88
B_In-C₃N₅	4.36
C₃N₅	5.80

Fig. 3. Band gap potential of pristine C3N5 (a), BC1-C3N5 (b), BN2-C3N5 (c), BN3-C3N5 (d), BN4-C3N5 (e), and BIn-C3N5 (f). Red, blue and magenta represent the contribution from N, C and B, respectively. (g) Band gap position of pristine C3N5 and other boron-doped C3N5 models.

Fig. 4. Optical absorption for boron-doped C3N5 and pristine C3N5 models.

Fig. 5. Adsorption energy for H2O and H2 molecule on different boron-doped C3N5 models and pristine C3N5. Blue and yellow represent H2O and H2 adsorption energies, respectively.

Fig. 6. Schematic of HER pathway for Volmer-Heyrovsky and Volmer-Tafel pathway in acidic (a) and alkaline (b) media on BN3-C3N5 model. The Tafel pathway is denoted with grey arrows and circles. The C, N, H, O, and boron atoms are represented in brown, grey, red, white, and green, respectively.

Fig. 7. Reaction kinetics for Volmer mechanism for boron-doped C3N5 and pristine C3N5 (a) and Volmer-Heyrovsky and Tafel mechanism for BN3-C3N5 and original C3N5 (b) in acid conditions. Tafel pathway is denoted in light grey. The inset of the Fig. is the reaction pathway on BN3-C3N5.

Fig. 8. Reaction kinetics for (a) Volmer mechanism of HER on BN3-C3N5 catalysts and (b) Volmer-Heyrovsky and Tafel mechanism of HER on BN3-C3N5 in alkaline condition. Tafel pathway is denoted in light grey. The right side of the Fig. is the schematic of the reaction mechanism on the catalyst surface. The inset of the Fig. is the reaction pathway on BN3-C3N5.

Fig. 9. Bader charge analysis on BN3-C3N5 (a), C3N5 (b), BIn-C3N5 (c), BC1-C3N5 (d), BN2-C3N5 (e), and BN4-C3N5 (f) models.

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2D氮化碳: 通过调节非金属硼掺杂C₃N₅阐明宽酸性及碱性pH范围的光催化析氢的反应机理

2D carbon nitrides: Regulating non-metal boron-doped C₃N₅ for elucidating the mechanism of wide pH range photocatalytic hydrogen evolution reaction

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[1]	赵彬彬, 钟威, 陈峰, 王苹, 别传彪, 余火根. 高晶化g-C₃N₄光催化剂: 合成、结构调控和光催化产氢[J]. 催化学报, 2023, 52(9): 127-143.
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[7]	刘博文, 蔡家杰, 张建军, 谭海燕, 程蓓, 许景三. MOF/CdS梯型光催化剂同时进行苯甲醇氧化和析氢反应及其机理研究[J]. 催化学报, 2023, 51(8): 204-215.
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